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<p>The advancement of flexible zinc-air batteries is constrained by the performance trade-off in their core component—alkaline hydrogel electrolytes—which often struggle to balance mechanical robustness with high ionic conductivity. To address this challenge, this study proposes a strategy of constructing multiple hydrogen-bonding networks induced by cellulose nanofibers (CNF) to design gel electrolytes that simultaneously exhibit superior mechanical durability and excellent hydroxide ion transport. Specifically, a polyvinyl alcohol (PVA)/CNF-based alkaline PVA/N-PAM/CNF hydrogel with a hydrogen-bond-rich architecture was successfully synthesized through in-situ polymerization of acrylamide (AM) within a PVA/CNF matrix, followed by a freeze-thaw cycling process. This uniquely engineered network endows the hydrogel with an exceptional ionic conductivity of 353.36 mS cm⁻¹, while also delivering outstanding mechanical properties, including a tensile strength of 690.55&#xa0;kPa, an elongation at break of 385.17%, and a toughness of 1.67&#xa0;MJ m⁻³. Furthermore, the incorporation of CNF significantly enhances the electrolyte’s alkali absorption capacity and water retention capability. When deployed in a flexible zinc-air battery, this PVA/N-PAM/CNF hydrogel electrolyte enables remarkable performance: a cycle life of 236 cycles, an energy density of 50.04 mW cm⁻², and an extended discharge duration of 938&#xa0;min.</p>

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Design of robust hydrogel electrolytes via cellulose nanofiber-induced hydrogen bonding for enhanced hydroxide transport

  • 期刊论文

  • 发表日期：

    2026年5月8日

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  • Hengyuan Dong,
  • Fanting Wu,
  • Jinshan Zhang,
  • Guotao Zhang,
  • Qiang Wang,
  • Weiliang Liu,
  • Hao Yu,
  • Cong Li,
  • Xiaoxia Cai,
  • Yanlin Sun

摘要

The advancement of flexible zinc-air batteries is constrained by the performance trade-off in their core component—alkaline hydrogel electrolytes—which often struggle to balance mechanical robustness with high ionic conductivity. To address this challenge, this study proposes a strategy of constructing multiple hydrogen-bonding networks induced by cellulose nanofibers (CNF) to design gel electrolytes that simultaneously exhibit superior mechanical durability and excellent hydroxide ion transport. Specifically, a polyvinyl alcohol (PVA)/CNF-based alkaline PVA/N-PAM/CNF hydrogel with a hydrogen-bond-rich architecture was successfully synthesized through in-situ polymerization of acrylamide (AM) within a PVA/CNF matrix, followed by a freeze-thaw cycling process. This uniquely engineered network endows the hydrogel with an exceptional ionic conductivity of 353.36 mS cm⁻¹, while also delivering outstanding mechanical properties, including a tensile strength of 690.55 kPa, an elongation at break of 385.17%, and a toughness of 1.67 MJ m⁻³. Furthermore, the incorporation of CNF significantly enhances the electrolyte’s alkali absorption capacity and water retention capability. When deployed in a flexible zinc-air battery, this PVA/N-PAM/CNF hydrogel electrolyte enables remarkable performance: a cycle life of 236 cycles, an energy density of 50.04 mW cm⁻², and an extended discharge duration of 938 min.